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In recent years, the power conversion efficiency (PCE) of perovskite solar cells (PSCs) has witnessed rapid progress. Nevertheless, the pervasive defects prone to non-radiative recombination and decomposition exist at the surface and the grain boundaries (GBs) of the polycrystalline perovskite films. Herein, we report a comprehensive dual-passivation (DP) strategy to effectively passivate the defects at both surface and GBs to enhance device performance and stability further. Firstly, a fluorinated perylene-tetracarboxylic diimide deriva